Sarmah, Smritakshi P.; Burlakov, Victor M.; Yengel, Emre; Banavoth, Murali; Alarousu, Erkki; El-Zohry, Ahmed M.; Yang, Chen; Alias, Mohd Sharizal; Zhumekenov, Ayan A.; Saidaminov, Makhsud I.; Cho, Nam Chul; Wehbe, Nimer; Mitra, Somak; Ajia, Idris A.; Dey, Sukumar; Mansour, Ahmed; Abdelsamie, Maged; Amassian, Aram; Roqan, Iman S.; Ooi, Boon S.; Goriely, Alain; Bakr, Osman; Mohammed, Omar F.(Nano Letters, American Chemical Society (ACS), 2017-02-01)[Article]
Understanding defect chemistry, particularly ion migration, and its significant effect on the surface’s optical and electronic properties is one of the major challenges impeding the development of hybrid perovskite-based devices. Here, using both experimental and theoretical approaches, we demonstrated that the surface layers of the perovskite crystals may acquire a high concentration of positively charged vacancies with the complementary negatively charged halide ions pushed to the surface. This charge separation near the surface generates an electric field that can induce an increase of optical band gap in the surface layers relative to the bulk. We found that the charge separation, electric field, and the amplitude of shift in the bandgap strongly depend on the halides and organic moieties of perovskite crystals. Our findings reveal the peculiarity of surface effects that are currently limiting the applications of perovskite crystals and more importantly explain their origins, thus enabling viable surface passivation strategies to remediate them.
Ugur, Esma; Sheikh, Arif D.; Munir, Rahim; Khan, Jafar Iqbal; Barrit, Dounya; Amassian, Aram; Laquai, Frédéric(ACS Energy Letters, American Chemical Society (ACS), 2017-07-31)[Article]
Planar perovskite solar cells can be prepared without high temperature processing steps typically associated with mesoporous device architectures; however, their efficiency has been lower and producing high quality perovskite films in planar devices has been challenging. Here, we report a modified two-step interdiffusion protocol suitable to prepare pin-hole free perovskite films with greatly improved morphology. This is achieved by simple addition of small amounts of glycol ethers to the preparation protocol. We unravel the impact the glycol ethers have on the perovskite film formation using in-situ UV-Vis absorbance and GIWAXS experiments. From these experiments we conclude: addition of glycol ethers changes the lead iodide to perovskite conversion dynamics and enhances the conversion efficiency, resulting in more compact polycrystalline films, and it creates micrometer-sized perovskite crystals vertically-aligned across the photoactive layer. Consequently, the average photovoltaic performance increases from 13.5% to 15.9% and reproduciability is enhanced, specifically when 2-methoxyethanol is used as additive.
Mottram, Alexander D.; Lin, Yen-Hung; Pattanasattayavong, Pichaya; Zhao, Kui; Amassian, Aram; Anthopoulos, Thomas D.(ACS Applied Materials & Interfaces, American Chemical Society (ACS), 2016-02-10)[Article]
Huang, Jing-Kai; Li, Mengliu; Wan, Yi; Dey, Sukumar; Ostwal, Mayur; Zhang, Daliang; Yang, Chih-Wen; Su, Chun-Jen; Jeng, U-Ser; Ming, Jun; Amassian, Aram; Lai, Zhiping; Han, Yu; Li, Sean; Li, Lain-Jong(ACS Nano, American Chemical Society (ACS), 2018-01-04)[Article]
Ultrathin two-dimensional (2D) polymeric layers are capable of separating gases and molecules based on the reported size exclusion mechanism. What is equally important but missing today is an exploration of the 2D layers with charge functionality, which enables applications using the charge exclusion principle. This work demonstrates a simple and scalable method of synthesizing a free-standing 2D coordination polymer Zn2(benzimidazolate)2(OH)2 at the air–water interface. The hydroxyl (−OH) groups are stoichiometrically coordinated and implement electrostatic charges in the 2D structures, providing powerful functionality as a charge barrier. Electrochemical performance of the Li–S battery shows that the Zn2(benzimidazolate)2(OH)2 coordination polymer layers efficiently mitigate the polysulfide shuttling effects and largely enhance the battery capacity and cycle performance. The synthesis of the proposed coordination polymeric layers is simple, scalable, cost saving, and promising for practical use in batteries.
LaGrow, Alec P.; Sinatra, Lutfan; Elshewy, Ahmed M.; Huang, Kuo-Wei; Katsiev, Khabiboulakh; Kirmani, Ahmad R.; Amassian, Aram; Anjum, Dalaver H.; Bakr, Osman(The Journal of Physical Chemistry C, American Chemical Society (ACS), 2014-08-21)[Article]
Faber, Hendrik; Lin, Yenhung; Thomas, Stuart R.; Zhao, Kui; Pliatsikas, Nikos; McLachlan, Martyn A.; Amassian, Aram; Patsalas, Panos A.; Anthopoulos, Thomas D.(ACS Applied Materials & Interfaces, American Chemical Society (ACS), 2015-01-14)[Article]
The use of ultrasonic spray pyrolysis is demonstrated for the growth of polycrystalline, highly uniform indium oxide films at temperatures in the range of 200-300 °C in air using an aqueous In(NO3)3 precursor solution. Electrical characterization of as-deposited films by field-effect measurements reveals a strong dependence of the electron mobility on deposition temperature. Transistors fabricated at ∼250 °C exhibit optimum performance with maximum electron mobility values in the range of 15-20 cm2 V -1 s-1 and current on/off ratio in excess of 106. Structural and compositional analysis of as-grown films by means of X-ray diffraction, diffuse scattering, and X-ray photoelectron spectroscopy reveal that layers deposited at 250 °C are denser and contain a reduced amount of hydroxyl groups as compared to films grown at either lower or higher temperatures. Microstructural analysis of semiconducting films deposited at 250 °C by high resolution cross-sectional transmission electron microscopy reveals that as-grown layers are extremely thin (∼7 nm) and composed of laterally large (30-60 nm) highly crystalline In2O3 domains. These unique characteristics of the In2O3 films are believed to be responsible for the high electron mobilities obtained from transistors fabricated at 250 °C. Our work demonstrates the ability to grow high quality low-dimensional In2O3 films and devices via ultrasonic spray pyrolysis over large area substrates while at the same time it provides guidelines for further material and device improvements.
Kim, Taesoo; Firdaus, Yuliar; Kirmani, Ahmad R.; Liang, Ru-Ze; Hu, Hanlin; Liu, Mengxia; El Labban, Abdulrahman; Hoogland, Sjoerd; Beaujuge, Pierre; Sargent, Edward H.; Amassian, Aram(ACS Energy Letters, American Chemical Society (ACS), 2018-05-03)[Article]
Realization of colloidal quantum dot (CQD)/organic photovoltaic (OPV) tandem solar cells that integrate the strong infrared absorption of CQDs with large photovoltages of OPVs is an attractive option toward high-performing, low-cost thin film solar cells. To date, monolithic hybrid tandem integration of CQD/OPV solar cells has been restricted due to the CQD ink’s catastrophic damage to the organic subcell, thus forcing the low bandgap CQD to be used as front cell. This sub-optimal configuration limits the maximum achievable photocurrent in CQD/OPV hybrid tandem solar cells. In this work, we demonstrate hybrid tandem solar cells employing a low-bandgap CQD back cell on top of an organic front cell thanks to a modified CQD ink formulation and a robust interconnection layer (ICL) which together overcome the long-standing integration challenges for CQD and organic subcells. The resulting tandem architecture surpasses previously reported current densities by ~20-25% and yields a state-of-the-art power conversion efficiency (PCE) of 9.4%.
Mansour, Ahmed; Dey, Sukumar; Amassian, Aram; Tanielian, Minas H.(ACS Applied Materials & Interfaces, American Chemical Society (ACS), 2015-07-22)[Article]
The unique optical and electrical properties of graphene have triggered great interest in its application as a transparent conducting electrode material and significant effort has been invested in achieving high conductivity while maintaining transparency. Doping of graphene has been a popular route for reducing its sheet resistance, but this has typically come at a significant cost in optical transmission. We demonstrate doping of few layers graphene with bromine as a means of enhancing the conductivity via intercalation without major optical losses. Our results demonstrate the encapsulation of bromine leads to air-stable transparent conducting electrodes with five-fold improvement of sheet resistance reaching at the cost of only 2-3% loss of optical transmission. The remarkably low tradeoff in optical transparency leads to the highest enhancements in the figure of merit reported thus far for FLG. Furthermore, we tune the workfunction by up to 0.3 eV by tuning the bromine content. These results should help pave the way for further development of graphene as a potential substitute to transparent conducting polymers and metal oxides used in optoelectronics, photovoltaics and beyond.
Kanimozhi, Catherine K.; Yaacobi-Gross, Nir; Chou, Kang Wei; Amassian, Aram; Anthopoulos, Thomas D.; Patil, Satish P.(Journal of the American Chemical Society, American Chemical Society (ACS), 2012-10-10)[Article]
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